GREEN CHEMISTRY
·
2024
·Vol. 26
·期 10
·6131-6138
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IF 9.3
Yan Wang,Xuan Wang,Yonghao Dong,Mingli Peng,Lina Guo,Mengyao Cui,Yuan He,Jiabao Yi,Huijun Ma,Huan Zhang,Haiming Fan
The selective oxidation of alcohols has drawn significant attention in heterogeneous catalysis with the increasing use of Pickering interfacial catalysis (PIC) for green transformations of alcohols. However, it is still highly desirable to design and develop a solid catalyst with easy separation and recycling, made from abundant resources through a simple synthesis route, for the selective oxidation of alcohols. In this study, ferrite nanoparticles, synthesized via a hydrothermal process, were employed to act as a stabilizer and catalyst in PIC for the oxidation of benzyl alcohol using H2O2. The ferrite nanoparticles exhibited higher catalytic performance in PIC than in acetonitrile. The turnover number (TON) of the nanocatalyst in PIC was found to be 1.5–4 times higher than that in acetonitrile, and the reaction constant in PIC (kPIC = 0.712 h−1) was almost twice that in acetonitrile (kCH3CN = 0.310 h−1) for MnFe2O4 nanoparticles. Moreover, other alcohols could also be oxidized with moderately high conversion and selectivity in PIC. Significantly, the ferrite nanocatalyst could be easily separated from PIC using a magnet for reuse, achieving 88% BzOH conversion after five cycles. The use of hazardous organic solvents was avoided in PIC, making it a more advanced, green and sustainable reaction system.
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RSC Advances
·
2024
·Vol. 14
·期 24
·16727-16735
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IF 3.9
Huizhong Wu,Qiong Yi,Xiang Li,Yingxi Wang,Ling Li
Low catalytic efficiency and catalyst recovery are the key factors limiting the practical application of advanced oxidation processes. In this work, a core–shell magnetic nanostructure Fe3O4@MIL-101(Fe, Co) was prepared via a simple solvothermal method. The core–shell structure and magnetic recovery performance were characterized by various technologies. The results of dye degradation experiments proved that within 10 minutes, the Fe3O4@MIL-101(Fe, Co)/PMS system can degrade more than 95% of 10 mg per L Rhodamine (RhB) at an initial pH of 7, which possesses higher catalytic activity than the Fe3O4/PMS system and the MIL-101(Fe, Co)/PMS system. The effects of initial solution pH and coexisting anions in water on the degradation of RhB were further discussed. The results showed that Fe3O4@MIL-101(Fe, Co) displayed excellent degradation efficiency in a wide pH range of 3–11 and capability of resisting coexisting anions. It is worth mentioning that after five cycles, the RhB removal rate can still be maintained at over 90% after 10 minutes of reaction. Free radical quenching experiments were further studied, confirming that ˙OH and SO4−˙ were involved in the degradation of RhB, while the dominating active free radical was SO4−˙. The possible reaction mechanism of the RhB degradation process was also inferred.
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Frontiers in Chemistry
·
2025
·
IF 4.2
Xianbing Zhang,Yuheng Liu,Jiajia Yuan
Metal-organic frameworks (MOFs) are recognized as important Fenton-like materials for environmental remediation. However, their applications are often hindered by slow cycling between Fe (III) and Fe (II). This study aimed to address the slow Fe (III)/Fe (II) cycling limitation of Fe-MOFs through dual modification strategy: bimetallic modification and amino functionalization. A series of NH2-MOF(Fe, Co) catalysts with varying Fe/Co ratios were synthesized via a hydrothermal method and evaluated for sulfamethoxazole (SMX) degradation. The optimized NH2-MOF(Fe, Co) catalyst (Fe/Co ratio = 7:3) exhibited substantially enhanced catalytic performance, with SMX removal rate and rate constant in the H2O2 system being 3.2 and 43.5 times higher than those of the Fe-MOF/H2O2 system, respectively. The catalyst demonstrated robust performance across a wide pH range (3.05–7.00), addressing a common limitation of Fenton-like systems. Physicochemical characterization revealed that the enhanced performance was attributed to two key factors: the synergistic effect between Co and Fe in the bimetallic active center, and improved electron transfer to the central metal due to -NH2 functionalization. These modifications effectively addressed the Fe (III)/Fe (II) redox cycling limitation. The proposed reaction mechanism provides insights into SMX degradation pathways in the NH2-MOF(Fe, Co)/H2O2 system. This study presents an efficient and stable MOF-based Fenton-like catalyst with potential applications in wastewater treatment and environmental remediation.
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Small
·
2025
·
IF 12.1
Jie Liu,Qiu Ye,Hui Liu,Junliang Chen,Yi Wu,Haoran Wang,Yunan Ye,Lei Zhang,Qipeng Li,Jinjie Qian
Transition metal sulfides (TMSs) have emerged as promising catalysts for the oxygen reduction reaction (ORR), yet achieving activity comparable to Pt-based benchmarks remains challenging. Herein, we present an in situ MOF-carbonization strategy to prepare transition metal-doped ZnS nanoparticles embedded in N, S-codoped carbon nanorods (M─ZnS/NSCNR, M═Fe, Co, Ni). Structural characterization confirms successful dopant integration into ZnS lattices within hierarchical carbon substrates, yielding enhanced defect density and optimal porosity. Furthermore, electrochemical evaluation reveals Fe─ZnS/NSCNR's exceptional ORR performance in 0.1 M KOH, exhibiting a half-wave potential of 0.897 V and limiting current density of 5.20 mA cm −2— surpassing both Pt/C and Co/Ni analogues. In zinc-air batteries, it can achieve a peak power density of 132.1 mW cm −2 , specific capacity of 685.6 mAh g Zn −1 , and minimal voltage gap (0.96 V) during 70 h cycling. DFT calculations show that transition metal doping effectively modulates the ZnS electronic structure by adjusting the position of the d-band center (d ε ). The Fe-doped ZnS model exhibits a well-balanced d ε value (−1.34 eV) and reduced OOH * adsorption barrier (0.62 eV), leading to enhanced ORR activity. This work establishes a scalable route for designing noble metal-free, MOF-derived ORR catalysts with superior activity-durability characteristics for advanced energy technologies.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2025
·
IF 5.4
Haozhe Li,Yufeng Sun,Zongtang Liu,Xinlong Sha,Zhenghao Fei,Lei Yu,Xiankun Wu,Xiaoju Wen,Rui Luo,Qihui Xu,Huiling Yan,Xiangdong Zhu,Binbin Qian
Nanoscale zerovalent iron (nZVI) has attracted extensive attention in the oxidative decomposition of organic matters as the persulfate (PS) activator due to its tunable physical/chemical properties and unique electronic structures. However, the trend of agglomeration and ease of oxidation for nZVI seriously hinder its further application. Herein, a composite catalyst composed of polyethyleneimine modified rice husk biochar (RHB-PEI) loaded with sulfide modified nZVI (S-nZVI) was constructed and its micro-structure was characterized by STEM, SEM, XRD, FT-IR and XPS. Results show that a layer of FeS shell with a thickness of ∼ 3 nm was formed around nZVI, and the whole core-shell structure was uniformly loaded on the N-doped RHB. The as-synthesized catalyst was used as a PS activator to remove sulfamethazine (SMT), a typical sulfonamide antibiotic. Compared with nZVI, the removal rate ( k obs ) of S-nZVI@RHB-PEI increased from 0.091 min⁻ 1 to 0.287 min⁻ 1 within 60 min, and the removal efficiency enhanced by 10.45 times in the fifth cycle experiment. The improvement of degradation performance in S-nZVI@RHB-PEI/PS system is not a simple accumulation caused by different heteroatom doping, but the synergistic effect from different heteroatom doping. The activation of PS by S-nZVI@RHB-PEI can effectively generate reactive oxygen species (ROS), including 1 O 2 , O 2 • ⁻, SO 4 • ⁻ and •OH, in which 1 O 2 played a major role. To be specific, under the attack of ROS, SMT was oxidized through a series of ring opening, SO 2 extrusion, Smiles rearrangement, and bond cleavage. This study verified the synergistic effect of N, S and Fe co-doped RHB on SMT degradation, the resultant catalyst demonstrated a higher electron transfer efficiency and thus exhibited excellent degradation efficiency and sustainable utilization over a wider pH range, which will advance the rational design of biochar supported nZVI catalysts and offer insights into the PS activation mechanism for the efficient degradation of SMT.
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Journal of Materials Chemistry A
·
2020
·Vol. 8
·期 48
·25919-25930
·
IF 11.301
Xiannong Tang,Rui Cao,Longbin Li,Bingyu Huang,Weijuan Zhai,Kai Yuan,Yiwang Chen
Developing precious-metal-free bifunctional oxygen reduction and evolution reaction (ORR/OER) electrocatalysts is of great significance for several key energy conversion and storage systems, yet remains a formidable challenge. Herein, we systematically designed Fe–Co–Ni trimetallic nanoalloys encapsulated in nitrogen-doped carbon nanotube@nanosheet frameworks (FeCoNi-NC) for application as effective bifunctional ORR/OER electrocatalysts. The rational structural design of FeCoNi-NC provides hierarchical porosity coupled with greatly increased effective electrochemical specific area for exposing abundant active sites and enhanced mass-transfer capability toward the ORR/OER. Experimental observations and theoretical calculations confirmed that Fe–Co–Ni nanoalloys interacting with pyridinic nitrogen-rich carbon synergistically optimized the adsorption/desorption free energies of oxygen intermediates, thus significantly enhancing the intrinsic ORR/OER activity. Consequently, FeCoNi-NC exhibits remarkable bifunctionality for the ORR (half-wave potential of 0.89 V) and OER (1.54 V at 10 mA cm−2) with ΔE = 0.65 V, and even outperforms Pt/C–RuO2 benchmarks. Moreover, the corresponding zinc–air battery shows large power density (315.2 mW cm−2), high capacity (803.78 mA h g−1 at 100 mA cm−2) and excellent cycling durability (over 100 hours at 50 mA cm−2), further testifying its practical applications. This work demonstrates an effective pathway to highly active non-precious-metal bifunctional catalysts toward sustainable energy technologies.
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ACS Applied Nano Materials
·
2026
·
IF 5.5
Xiaoyang Dong,Jinxing Wang,Jingdong Yang,Wen Zeng,Guangsheng Huang,Jingfeng Wang
Magnesium (Mg)–air batteries are regarded as promising large-scale energy-storage devices because of their high theoretical energy density, low material cost, intrinsic safety, and environmental benignity. Nevertheless, their practical deployment is severely hindered by sluggish oxygen reduction reaction (ORR) kinetics at the cathode. Herein, nanoscale transition-metal–nitrogen-doped carbon (M-N-C, M = Fe, Co, Ni) electrocatalysts─denoted FNC, CNC, and NNC─are prepared by argon-pyrolysis of Prussian blue analogues (PBAs). The cationic and anionic ligands are systematically varied to tailor the crystal phase, pore architecture, and nanoscale M-Nx coordination environment. Comprehensive characterization shows that CNC possesses the highest density of well-dispersed Co-Nx active nanosites embedded in a graphitic matrix. This ensures rapid electron transfer and abundant accessible active centers. Electrochemical tests in alkaline (0.1 M KOH) and neutral (3.5 wt % NaCl) electrolytes demonstrate that CNC delivers the most robust ORR activity and stability (CNC > FNC > NNC) via a near-ideal 4 e pathway. Meanwhile, CNC exhibits better stability than commercial Pt/C in both alkaline and neutral electrolytes. As the cathode nanocatalyst in Mg-air batteries, CNC is found to yield a peak power density of 19.14 mW/cm2─only 0.66 mW/cm2 below that of commercial Pt/C. The decisive role of nanoscale M-Nx coordination environments in boosting ORR kinetics is thus elucidated. This work provides a nanomaterials-driven strategy for developing high-performance, cost-effective electrocatalysts for Mg-air batteries.
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INTERNATIONAL JOURNAL OF REFRACTORY METALS & HARD MATERIALS
·
2020
·
IF 3.407
Zhonghua Li,Faqiang Shi,Limeng Liu,Jozef Vleugels,Shuigen Huang
TaC x (x = 0.5, 0.55, 0.6, 0.7) ceramics with 20 mol% Fe, Co or Ni addition were prepared by hot pressing TaC and Ta powder mixtures at 1800 °C. X-ray diffraction, scanning electron microscopy, transmission electron microscopy , high resolution transmission electron microscopy , X-ray energy dispersive spectroscopy and selected area electron diffraction were used to investigate the constituent phases and microstructures of the composites. Vickers hardness , flexural strength and fracture toughness were measured. Intermetallic compounds Fe 7 Ta 3 , Co 2 Ta and Ni 3 Ta were formed due to reactions of Fe, Co and Ni with Ta. The remaining TaC and Ta reacted to form hexagonal Ta 2 C, rhombohedral ζ-Ta 4 C 3-z or cubic TaC y depending on the overall C:Ta ratios. The microstructure of the TaC 0.5 –20 mol% Fe, Co, Ni compositions (where C:Ta = 0.5) were composed of intermetallics and fine anisotropic Ta 2 C and ζ-Ta 4 C 3-z grains. As the C:Ta ratio increased to 0.55–0.7, the ζ-Ta 4 C 3-z and TaC y grains were enlarged in size and equiaxed in the TaC 0.55 -, TaC 0.6 -, and TaC 0.7 –20 mol% Fe, Co, Ni compositions. Addition of Ni instead of Fe and Co benefitted to refine microstructures of the composites. The TaC 0.5 –20 mol% Fe, Co, Ni compositions had good flexural strength (580-650 MPa) and fracture toughness (9.3–9.5 MPa·m 1/2 ) due to growth of fine lamellar grains, despite the high Ta 2 C content.
研究领域:
材料科学
·
陶瓷
·
显微结构
·
力学性能
·
相变
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Tingting Ge,Hui Guo,Cuncun Zuo,Yanxia Zheng,Shuyue Li,Haofei Huang,Ming Wang,Guangjun Cui,Xinpeng Guo,Yuchao Li
Series of magnetic metal-doped cerium oxide (MCeO x , M = Fe, Co and Ni) were synthesized and applied to support nano-gold (Au) as catalyst for synthesis of methyl methacrylate (MMA) through gas-liquid-solid three-phase oxidation esterification of methacrolein (MAL) and methanol (MeOH). Hydrothermal synthesis method was applied for MCeO x preparation and deposition-precipitation method was for nano-Au supported catalyst. The catalysts were characterized through XRD, H 2 -TPR, NH 3 -TPD, FT-IR, TG, BET, TEM-EDS and VSM. Results showed that Au/FeCeO x had strong magnetic properties and could be easily separated by external magnetism. Moreover, the doping of Fe could improve the redox properties and acidic sites of the catalyst. Catalyst performances were evaluated in a micro batch reactor. 5% - Au/FeCeO x allowed the highest reaction activity to be observed with MAL conversion of 80.2% and MMA selectivity of 96.1%. Surface catalytic reaction mechanism on Au/CeO 2 was established and transition states of oxidative esterification were obtained using density functional theory (DFT). Magnetically recoverable nano-Au/FeCeO x catalysts maintain stable activity after 5 cycles, which makes it a promising catalyst for industrial application.
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NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 23
·11242-11254
·
IF 3.925
Lihong Tao,Jun Chen,Jianjun Zhao,Sydorov Dmytro,Qian Zhang,Shengwen Zhong
In view of the disadvantage of the limited active site utilization due to the easy aggregation of phthalocyanine compounds, three kinds of graphene composite metal phthalocyanines (TN-MPc@GN, M = Fe, Co, Ni) were prepared using an in situ composite method, and their electrochemical properties were investigated as anode materials for lithium-ion batteries. The layered structure and large specific surface area of graphene are used to disperse phthalocyanine uniformly, so that the conjugated structure (CC/CN/NO) of phthalocyanine is more exposed and the utilization of active sites for embedding lithium ions are greatly enhanced. At the same time, the large surface area is beneficial to the contact between materials and the electrolyte, which results in a faster transmission path. As a result, the first discharge specific capacities of the graphene composite phthalocyanine (TN-MPc@GN, M = Fe, Co, Ni) electrodes are 440.8, 765.0 and 753.9 mA h g−1, respectively. After 420 cycles, the specific capacities increased to 734.6, 844.7 and 949.1 mA h g−1, respectively, which are much higher than those of the pristine three phthalocyanine (TN-MPC, M = Fe, Co, Ni) electrodes without the graphene composite. Using the graphene composite can be an effective strategy to improve the utilization of active sites of organic electrode materials in lithium-ion batteries.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Xiwen Tao,Zhengguang Zhang,Zheng Li,Shuangsheng Xiong,Shengmei Wang,Faming Gao,Chen Wang,Li Hou
Potassium-ion batteries (PIBs) have become the desirable alternatives for lithium-ion batteries (LIBs) originating from abundant reserves and appropriate redox potential, while the considerable radius size of K+ leading to poor reaction kinetics and huge volume expansion limits the practical application of PIBs. Hybridization of transition-metal phosphides and carbon substrates can effectively optimize the obstacles of poor conductivity, sluggish kinetics, and huge volume variation. Thus, the peapod-like structural MxPy@BNCNTs (M = Fe, Co, and Ni) composites as anode materials for PIBs were synthesized through a facile strategy. Notably, the unique architecture of B/N codoped carbon nanotube array as fast ion/electron transfer pathways effectively improves the electronic conductivity of composites. The MxPy nanoparticles (NPs) are encapsulated in BNCNTs with an amorphous carbon layer (5–10 nm), which discernibly alleviate the volume changes during potassiation/depotassiation. In conclusion, the composites show a commendable cycling performance, possessing reversible capacities of 111, 152, and 122 mA h g–1 after 1000 cycles at 1.0 A g–1 with a negligible capacity loss for FeP@BNCNT, CoP/Co2P@BNCNT, and Ni2P@BNCNT electrodes, respectively. Especially, after 1000 cycles at 2.0 A g–1, the CoP/Co2P@BNCNT electrode still possesses a capacity of 87.9 mA h g–1, demonstrating excellent rate performance and long-term life. This work may offer an innovative and viable route to construct a stable architecture for solving the issue of poor stability of TMP-based anodes at a high current density.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Weicun Jiang,Yaling Li,Yunshi Xu,Ting Jiang,Mingyu Zhao,Mengyuan Deng,Rongliang Wu,Yi Wang
Rational design of hierarchically structured carbon nanomaterials and also the facile regulation of their metal species decoration for enhanced oxygen reduction reaction (ORR) are urgently required. Herein, N-doped carbon nanospheres (N-MCN) with plentiful pyridinic and graphitized N-induced active sites were closely bridged with carbon nanotubes to remedy the conductivity loss of N-doping. The as-obtained N-MCN@CNT exhibited hierarchically porous structure with large surfaces area and good conductivity with small charge transfer resistance, which therefore had a superior ORR activity to the other carbon-base catalysts. Importantly, the metal species (M = Fe or Co) can be loaded in this porous N-MCN@CNT via a simple co-pyrolysis, where their numbers and shapes can be easily regulated. It was found the optimal adsorption of metal ions into the precursors produced both single atom and few carbon-coated nanoparticles in M/N-MCN@CNT, which thus synergistically contributed the enhanced ORR performances, including large current density, low onset and half-wave potentials, as well as superior stability and methanol tolerance than those of commercial 20 wt% Pt/C. Moreover, M/N-MCN@CNT also demonstrated comparable oxygen evolution reaction activity to RuO 2 possibly due to the regulated metal species. This work provided a strategy to regulate the nanostructure and intrinsic active sites of carbon-based electrocatalysts.
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